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Subject: Garnets × WGL Institute: MBI ×

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    Tm3+-doped calcium lithium tantalum gallium garnet (Tm:CLTGG): novel laser crystal
    (Washington, DC : OSA, 2021) Alles, Adrian; Pan, Zhongben; Loiko, Pavel; Serres, Josep Maria; Slimi, Sami; Yingming, Shawuti; Tang, Kaiyang; Wang, Yicheng; Zhao, Yongguang; Dunina, Elena; Kornienko, Alexey; Camy, Patrice; Chen, Weidong; Wang, Li; Griebner, Uwe; Petrov, Valentin; Solé, Rosa Maria; Aguiló, Magdalena; Díaz, Francesc; Mateos, Xavier
    We report on the development of a novel laser crystal with broadband emission properties at ∼2 µm – a Tm3+,Li+-codoped calcium tantalum gallium garnet (Tm:CLTGG). The crystal is grown by the Czochralski method. Its structure (cubic, sp. gr. 𝐼𝑎3¯𝑑, a = 12.5158(0) Å) is refined by the Rietveld method. Tm:CLTGG exhibits a relatively high thermal conductivity of 4.33 Wm-1K-1. Raman spectroscopy confirms a weak concentration of vacancies due to the charge compensation provided by Li+ codoping. The transition probabilities of Tm3+ ions are determined using the modified Judd-Ofelt theory yielding the intensity parameters Ω2 = 5.185, Ω4 = 0.650, Ω6 = 1.068 [10−20 cm2] and α = 0.171 [10−4 cm]. The crystal-field splitting of the Tm3+ multiplets is revealed at 10 K. The first diode-pumped Tm:CLTGG laser generates 1.08 W at ∼2 µm with a slope efficiency of 23.8%. The Tm3+ ions in CLTGG exhibit significant inhomogeneous spectral broadening due to the structure disorder (a random distribution of Ta5+ and Ga3+ cations over octahedral and tetrahedral lattice sites) leading to smooth and broad gain profiles (bandwidth: 130 nm) extending well above 2 µm and rendering Tm:CLTGG suitable for femtosecond pulse generation.
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    Dissecting spin-phonon equilibration in ferrimagnetic insulators by ultrafast lattice excitation
    (Washington, DC [u.a.] : Assoc., 2018) Maehrlein, Sebastian F.; Radu, Ilie; Maldonado, Pablo; Paarmann, Alexander; Gensch, Michael; Kalashnikova, Alexandra M.; Pisarev, Roman V.; Wolf, Martin; Oppeneer, Peter M.; Barker, Joseph; Kampfrath, Tobias
    To gain control over magnetic order on ultrafast time scales, a fundamental understanding of the way electron spins interact with the surrounding crystal lattice is required. However, measurement and analysis even of basic collective processes such as spin-phonon equilibration have remained challenging. Here, we directly probe the flow of energy and angular momentum in the model insulating ferrimagnet yttrium iron garnet. After ultrafast resonant lattice excitation, we observe that magnetic order reduces on distinct time scales of 1 ps and 100 ns. Temperature-dependent measurements, a spin-coupling analysis, and simulations show that the two dynamics directly reflect two stages of spin-lattice equilibration. On the 1-ps scale, spins and phonons reach quasi-equilibrium in terms of energy through phonon-induced modulation of the exchange interaction. This mechanism leads to identical demagnetization of the ferrimagnet’s two spin sublattices and to a previously inaccessible ferrimagnetic state of increased temperature yet unchanged total magnetization. Finally, on the much slower, 100-ns scale, the excess of spin angular momentum is released to the crystal lattice, resulting in full equilibrium. Our findings are relevant for all insulating ferrimagnets and indicate that spin manipulation by phonons, including the spin Seebeck effect, can be extended to antiferromagnets and into the terahertz frequency range.